Made available in DSpace on 2015-03-03T15:16:25Z (GMT). No. of bitstreams: 1 EdvanM_TESE.pdf: 3369226 bytes, checksum: 764b7a9d291d433b871e24f1776af89d (MD5) Previous issue date: 2011-07-29 / Coordena??o de Aperfei?oamento de Pessoal de N?vel Superior / In this work we present a study for the structural, electronic and optical properties, at ambient conditions of SrSnO3, SrxBa1?xSnO3 (x = 0:2; 0:4; 0:6; 0:8) and BaSnO3 crystals, all of them member of perovskite-type earth stannates class, ASnO3. The theoretical model employed was based on the density functional theory (DFT), considering both the local density and the generalized gradient approximations, LDA-CAPZ and GGA-PBE (OPIUM), respectively. For orthorhombic SrSnO3, the electronic band structure, density of states, complex dielectric function, optical absorption, and the infrared and Raman spectra were computed. Calculated lattice parameters are closed to the experimental measurements, and an indirect band gap E(S -> t ?)=1.97 eV (2.27 eV) was obtained within the GGA (LDA) level of calculation. E ective masses for holes and electrons were estimated, being very anisotropic in comparison with similar results for orthorhombic CaSnO3. The complex dielectric function and the optical absorption of SrSnO3 are sensitive to the plane of polarization of the incident light. The infrared spectrum between 100-600 cm-?1 was obtained, with its main peaks being assigned, and a good agreement between experimental and theoretical peaks of the Raman spectrum of orthorhombic SrSnO3 was achieved. For SrxBa1?xSnO3 series, their electronic properties were investigated. The cubic Sr0:2Ba0:8SnO3 has an indirect band gap, while tetragonal Sr0:4Ba0:6SnO3, orthorhombic Sr0:6Ba0:4 SnO3 and Sr0:8Ba0:2SnO3 exhibit a direct band gap. The Kohn-Sham minimum electronic band gap oscillates of 2.62 eV (tetragonal Sr0:4Ba0:6SnO3, LDA) to 1.52 eV (orthorhombic Sr0:6Ba0:4Sn O3, LDA). The effective masses for holes and electrons were estimated, being anisotropic in the series. For cubic BaSnO3, the electronic band structure, density of states, dielectric function and optical absorption were calculated, as well as the infrared absorption spectra after computing the vibrational modes of the crystal at q = 0. Dielectric optical permittivities and polarizabilities at w = 0 and w = ?? were also obtained. An indirect band gap E(R -> T?) of 1.01 eV and 0.74 eV was achieved within the LDA-CAPZ and the GGA-PBE, respectively, which is smaller than the experimental data ( ?? 3.1 eV). Effective masses of holes and electrons were estimated by parabolic tting along di erent directions at the valence band maximum and conduction band minimum, being highly isotropic for electrons and anisotropic for holes, allowing us to suggest that indirect gap cubic BaSnO3 is a semiconductor with potential for optoelectronic applications. The optical properties reveal a degree of isotropy for the crystal with respect to di erent polarization planes of incident light. The infrared spectrum between 100-600 cm?-? was obtained, with its main peaks being assigned / Apresentamos neste trabalho um estudo das propriedades estruturais, eletr?nicas e ?pticas, em temperatura ambiente dos cristais de SrSnO3, SrxBa1xSnO3 (x = 0:2; 0:4; 0:6; 0:8) e BaSnO3, todos eles membros da classe das perovskitas do tipo estanatos terrosos, ASnO3. O nosso modelo te?rico foi baseado na teoria do funcional da densidade (DFT) considerando as aproxima??es da densidade local e do gradiente generalizado, LDA-CAPZ e GGA-PBE (OPIUM), respectivamente. Para o SrSnO3 ortor?mbico, foram calculadas a estrutura de bandas eletr?nica, densidade de estados, fun??o diel?trica complexa, absor??o ?ptica e os espectros infravermelho e Raman. Os par?metros de rede calculados est?o pr?ximos dos resultados experimentais, e um band gap indireto E(S !)=1.97 eV (2.27 eV) foi obtido dentro do n?vel GGA (LDA) de c?lculo. As massas efetivas dos buraco e dos el?trons foram estimadas, sendo elas muito anisotr?picas em compara??o com os resultados similares para o CaSnO3 ortor?mbico. Al?m disso, nossos resultados mostram que a fun??o diel?trica complexa e a absor??o ?ptica do SrSnO3 s?o sens?veis ao plano de polariza??o da luz incidente. O espectro infravermelho entre 100{600 cm1 foi obtido, com seus principais picos sendo assinalados, e uma boa concord?ncia dos resultados experimentais e te?ricos do espectro Raman do SrSnO3 ortor?mbico foram alcan?ados. Para a s?rie SrxBa1xSnO3, as propriedades eletr?nicas foram investigadas. O Sr0:2Ba0:8 SnO3 c?bico possui um band gap indireto, enquanto o Sr0:4Ba0:6SnO3 tetragonal, os ortor?mbicos Sr0:6Ba0:4SnO3 e Sr0:8Ba0:2SnO3 exibem um band gap direto. O band gap eletr?nico m?nimo de Kohn-Sham oscila de 2.62 eV (Sr0:4Ba0:6SnO3 tetragonal, LDA) at? 1.52 eV (Sr0:6Ba0:4SnO3 ortor?mbico, LDA). As massas efetivas de buracos e de el?trons foram estimadas, sendo anisotr?picas nas s?ries. vi Para o BaSnO3 c?bico, foram calculadas a estrutura de bandas eletr?nica, densidade de estados, fun??o diel?trica e absor??o ?ptica, bem como o espectro infravermelho de absor??o ap?s computar os modos de vibra??o do cristal em q = 0. A permissividade ?ptica diel?trica e as polarizabilidades em ! = 0 e ! = 1 foram obtidas. Um band gap indireto E(R !) de 1.01 eV e 0.74 eV foi obtido com o LDA-CAPZ e o GGA-PBE, respectivamente, que ? menor que o dado experimental (3.1 e V). As massas efetivas de buraco e de el?tron foram estimadas atrav?s de um ajuste parab?lico ao longo de diferentes dire??es no m?ximo da banda de val?ncia e no m?nimo da banda de condu??o, sendo muito isotr?pico para el?trons e anisotr?pico para buracos, permitindo-nos sugerir que o BaSnO3 c?bico de gap indireto ? um semicondutor com potencial para aplica??es optoeletr?nicas. As propriedades ?pticas revelaram um grau de isotropia para o cristal com respeito aos diferentes planos de polariza??o de luz incidente. O espectro infravermelho entre 100{600 cm 1 foi obtido, com seus principais picos sendo assinalados

In dieser Arbeit werden das Wachstum und die Charakterisierung der Heterostruktur eines FeFET auf der Grundlage von BaSnO3, LaInO3 und (K,Na)NbO3 Schichten untersucht. Für jedes Material wurden die Wachstumsbedingungen bestimmt und im Hinblick auf die strukturellen und elektrischen Eigenschaften optimiert. Epitaktische BaSnO3 Filme, die auf SrTiO3 Substraten gewachsen sind, weisen eine hohe Dichte an Versetzungen auf, die ihre elektrischen Eigenschaften beeinträchtigen. Die Verwendung von NdScO3 Substraten und Einführung einer SrSnO3 Pufferschicht verbesserten die strukturellen und elektrischen Eigenschaften der BaSnO3 Schichten. Dies ermöglichte schließlich Untersuchungen an der LaInO3/BaSnO3 Grenzfläche. Schon eine geringe La-Dotierung der BaSnO3 Schicht von 0,3 % führte zur Bildung eines 2DEG nach der Grenzflächenbildung und damit zum Einschluss von Elektronen an der Grenzfläche. Dies konnte durch C-V, Van-der-Pauw und Hall-Effekt-Messungen eindeutig nachgewiesen werden. Eine deutliche Verbesserung der strukturellen und elektrischen Eigenschaften der BaSnO3 Schichten wurde durch die Verwendung von LaInO3:Ba Substraten erreicht. Diese sind gitterangepasst an BaSnO3, sodass zum ersten Mal vollständig verspannte Schichten ohne Versetzungen gewachsen werden konnten. Strukturelle und elektrische Eigenschaften von (K,Na)NbO3 Schichten wurden auf SrRuO3/DyScO3 und SrTiO3:Nb-Substraten untersucht. Auf diese Weise wurden der Einfluss der Gitterdehnung auf die kritische Schichtdicke und die Prozesse der plastischen Relaxation des Gitters bestimmt. Die elektrische Charakterisierung ergab einen hohen Leckstrom, der durch strukturelle Defekte verursacht wird. Die gesamte FeFET Heterostruktur wurde auf LaInO3:Ba Substraten gewachsen und untersucht. BaSnO3 und LaInO3 Schichten wuchsen kohärent, während (K,Na)NbO3 Schichten eine plastische Gitterrelaxation aufwiesen. Das führte zur Bildung von Strukturdefekten und zu einer Verschlechterung der ferroelektrischen Eigenschaften. / In this thesis, the design, growth and characterisation of the heterostructure of a FeFET based on BaSnO3, LaInO3 and (K,Na)NbO3 thin films are investigated. For each material, the growth conditions were determined and optimised with respect to their structural and electrical properties. Epitaxial BaSnO3 thin films grown on SrTiO3 substrates exhibit a high density of threading dislocations, which degrade their electrical properties. The use of NdScO3 substrates and the introduction of a SrSnO3 buffer layer improved the structural and electrical properties of the BaSnO3 thin films. This finally allowed investigations on the LaInO3/BaSnO3 heterointerface. Even a low La doping of the BaSnO3 layer of 0.3 % led to the formation of a 2DEG after interface formation and thus to the confinement of electrons at the interface. This could be clearly demonstrated by C-V, Van-der-Pauw and Hall effect measurements. A significant improvement of the structural and electrical properties of the BaSnO3 thin films was achieved by using LaInO3:Ba substrates. These are lattice-matched to BaSnO3 so that, for the first time, fully strained thin films could be grown without dislocations. Structural and electrical properties of (K,Na)NbO3 thin films were investigated on SrRuO3/DyScO3 and SrTiO3:Nb substrates. In this way, the influence of lattice strain on the critical film thickness and plastic lattice relaxation were determined. Their electrical characterisation revealed a high leakage current caused by structural defects. Therefore, the entire FeFET heterostructure was grown and investigated on LaInO3:Ba substrates. The BaSnO3 and LaInO3 thin films were grown coherently, while the (K,Na)NbO3 thin films exhibited plastic lattice relaxation. This led to the formation of structural defects and consequently to a deterioration of their ferroelectric properties.